To remedy the widespread chromium (Cr) pollution in the environment, this study mainly used the ultrasonic-assisted co-precipitation and precipitation methods to prepare FeS-modified Fe-Al-layered double hydroxide (FeS/LDH) composite material. The experimental results showed that FeS/LDH has higher removal efficiency of Cr in aqueous solution and stronger anti-interference ability than unmodified LDH. Under the same reaction conditions, the removal efficiency of total Cr(Cr(T)) using LDH was 34.85%, and the removal efficiency of Cr(VI) was 46.76%. For FeS/LDH, the removal efficiency of Cr(T) and Cr(VI) reached 99.57% and 100%, respectively. The restoration of Cr(T) and Cr(VI) by FeS/LDH satisfied the Langmuir adsorption isotherm. The maximum adsorption capacity of Cr(T) and Cr(VI) achieved 102.9 mg/g and 147.7 mg/g. The efficient removal of Cr by FeS/LDH was mainly based on the triple synergistic effect of anion exchange between Cr(VI) and interlayer anions, redox of Cr(VI) with Fe2+ and S2−, and co-precipitation of Fe3+ and Cr3+.